基于壳聚糖物理网络的高强韧双网络水凝胶的构建、调控与应用

doi:10.6023/A20080370

化学学报 ›› 2021, Vol. 79 ›› Issue (1): 1-9.DOI: 10.6023/A20080370 上一篇下一篇

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基于壳聚糖物理网络的高强韧双网络水凝胶的构建、调控与应用

杨艳宇^a^,^b, 王星^b^,^*(), 吴德成^b^,^c^,^*()

a 郑州大学材料科学与工程学院郑州 450001)
(
b 中国科学院化学研究所北京 100190)
(
c 南方科技大学生物医学工程系深圳 518055

投稿日期:2020-08-16 发布日期:2020-09-16
通讯作者: 王星, 吴德成

作者简介:

杨艳宇, 2017年博士毕业于中国科学院化学研究所, 高分子化学与物理专业, 导师为吴德成研究员, 现为郑州大学副教授, 研究方向为高机械性能水凝胶材料的构筑与功能化研究.

王星, 中国科学院化学研究所副研究员, 2014年于中国科学院化学研究所取得博士学位, 研究方向为医用高分子水凝胶的可控制备、功能构筑及应用研究.

吴德成, 中国科学院化学研究所研究员、南方科技大学生物医学工程系讲席教授. 研究方向为生物医用高分子、医用敷料/耗材、生物成像、药物输运和组织工程.

* E-mail: wangxing@iccas.ac.cn; dcwu@iccas.ac.cn

基金资助:
国家自然科学基金(Nos. 51803188); 国家自然科学基金(51973226); 国家自然科学基金(21725403)

Chitosan-Based High-Mechanical Double-Network Hydrogels: Construction, Modulation and Applications

Yanyu Yang^a^,^b, Xing Wang^b^,^*(), Decheng Wu^b^,^c^,^*()

a College of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, China)
(
b Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China)
(
c Department of Biomedical Engineering, Southern University of Science and Technology, Shenzhen 518055, China

Received:2020-08-16 Published:2020-09-16
Contact: Xing Wang, Decheng Wu
Supported by:
the National Natural Science Foundation of China(Nos. 51803188); the National Natural Science Foundation of China(51973226); the National Natural Science Foundation of China(21725403)

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摘要/Abstract

双网络水凝胶由两个具有相反物理性质的交联网络构成, 硬而脆的第一网络在变形过程中断裂耗散能量, 从而增韧凝胶. 当第一网络为具有重建能力的物理网络时, 双网络水凝胶表现出优异的抗软化和机械稳定性. 目前双网络水凝胶第一物理网络类型单一、结构和力学调控繁琐, 因而其开发和应用受到限制. 针对上述问题, 作者发展了硬而脆的壳聚糖物理网络构建的新策略, 壳聚糖的网络类型、结构和物理性质均能简便调控, 然后将其作为第一网络成功地制备了多种高强韧且结构性能可灵活调控的双网络水凝胶, 在抗冻敷料、生物医用、柔性电子和可穿戴设备等领域具有重要的应用价值. 构建壳聚糖基双网络水凝胶的策略操作简单、普适通用, 能够有力促进高强韧水凝胶的开发、功能化及应用.

关键词: 壳聚糖物理网络, 高强韧水凝胶, 结构和性能调控, 耐冻性, 柔性可穿戴设备

Double-network (DN) hydrogels are composed of two asymmetric networks with contrasting properties, wherein the rigid and brittle network serving as sacrificial bonds effectively dissipates energy to enhance the mechanical performance. The first reconstructable physical network endows the DN hydrogels with outstanding anti-soften and mechanical stability. However, the monotonous type of physical networks and the difficulty in tailoring structure and mechanics greatly limit the development and application of DN hydrogels. Focusing on these problems, we have fabricated the rigid and brittle chitosan physical network with adjustable network type, structure and property and further constructed various chitosan-based DN hydrogels with high mechanical performance and tunable mechanics. The hydrogels were potential materials for anti-freezing dresses, biomedical materials, flexible electronics and wearable devices. The universal strategy of constructing chitosan-based DN hydrogels was beneficial for developing various functional and high-mechanical hydrogels and broadening their applications.

Key words: chitosan physical network, strong and tough hydrogel, structural and mechanical regulation, freezing tolerance, flexible wearable device

引用此文

杨艳宇, 王星, 吴德成. 基于壳聚糖物理网络的高强韧双网络水凝胶的构建、调控与应用[J]. 化学学报, 2021, 79(1): 1-9.

Yanyu Yang, Xing Wang, Decheng Wu. Chitosan-Based High-Mechanical Double-Network Hydrogels: Construction, Modulation and Applications[J]. Acta Chimica Sinica, 2021, 79(1): 1-9.

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图/表 12

图1. 壳聚糖基双网络水凝胶的高机械性能、结构调控性及应用

Figure 1. The high mechanical performance, tunable structure and applications of chitosan-based DN hydrogel

图2. 壳聚糖的结构式

Figure 2. Structure of chitosan chain

图3. 多层结构的壳聚糖结晶网络凝胶[9]

Figure 3. Multi-membrane chitosan crystal network hydrogel[9]

图4. 壳聚糖离子网络凝胶[11]

Figure 4. Scheme of chitosan ionic network hydrogel[11]

图5. 壳聚糖-聚丙烯酰胺微晶-共价双网络水凝胶的制备示意图[12]

Figure 5. Scheme of fabrication of chitosan-polyacrylamide microcrystalline-covalent DN hydrogel[12]

图6. 壳聚糖-聚丙烯酰胺微晶-共价双网络水凝胶优异的(A)负重能力、(B)抗碾压性、(C)缺口不敏感性、(D)能量耗散和(E)自恢复性能[12]

Figure 6. Mechanical performance of chitosan-polyacrylamide microcrystalline-covalent DN hydrogel: (A) load-bearing capacity, (b) rolling resistance, (C) crack blunting, (D) energy dissipation and (E) self-recoverability[12]

图7. 壳聚糖-聚丙烯酰胺链缠结-共价水凝胶的(A)制备示意图和(B, C)溶胀行为[12]

Figure 7. (A) Scheme of fabrication of chitosan-polyacrylamide chain-entanglement-covalent DN hydrogel and (B, C) its swelling behavior in water[12]

图8. 壳聚糖-聚丙烯酰胺离子-共价双网络水凝胶的(A)结构示意图、(B)高弹性、(C)溶胀行为及(D, E)溶胀前后的机械性能对比[20]

Figure 8. (A) Structure and (B) high elasticity of chitosan-polyacrylamide ionic-covalent DN hydrogel. (C) Swelling behavior and (D, E) mechanical performance of the original and swollen hydrogel[20]

图9. 水凝胶结构和性能的灵活调控[20]

Figure 9. Flexible adjustment of structure and mechanics of hydrogel[20]

图10. 高强韧导电抗冻的壳聚糖基双网络水凝胶的(A)能量耗散机制、(B)离子导电机理和(C)抗冻机理[27]

Figure 10. (A) Energy dissipation mechanism, (B) ionic conductivity and (C) anti-freezing performance of high-mechanical chitosan-based DN hydrogel[27]

图11. 壳聚糖-聚羟乙基丙烯酰胺双网络水凝胶作为皮肤的防冻材料. (A)冻伤模型示意图; 移除冷硬币之后的(B)皮肤、(C)硬币(上)及水凝胶(下)的照片; 皮肤组织学显微镜图像: (D)未被保护的皮肤、(E)被复合水凝胶和(F)被双网络水凝胶保护的皮肤[27]

Figure 11. CS-PHEAA DN hydrogel as ant-freezing dressing to protect skin from frostbite. (A) Schematic diagram of frostbite model. Photos of (B) skin, (C) cold coins (top) and hydrogels (bottom) after coving the cold coin for 30 s. Histological microscopy images of (D) bare skin, (E) skin protected by composite hydrogel and (F) skin protected by DN hydrogel[27]

图12. 壳聚糖基双网络水凝胶作为多模式抗冻可穿戴设备检测人体活动[27- 28]

Figure 12. Chitosan-based DN hydrogel serving as anti-freezing and multi-model wearable device to detect various human motions[27- 28]

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基于壳聚糖物理网络的高强韧双网络水凝胶的构建、调控与应用

Chitosan-Based High-Mechanical Double-Network Hydrogels: Construction, Modulation and Applications

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